A combined lidar-photometer method that permits the retrieval of vertical profiles of ash and non-ash (fine-mode) particle mass concentrations is presented. By using a polarization lidar, the contributions of non-ash and ash particles to total particle backscattering and extinction are separated. Sun photometer measurements of the ratio of particle volume concentration to particle optical thickness (AOT) for fine and coarse mode are then used to convert the non-ash and ash extinction coefficients into respective fine-mode and ash particle mass concentrations. The method is applied to European Aerosol Research Lidar Network (EARLINET) and Aerosol Robotic Network (AERONET) Sun photometer observations of volcanic aerosol layers at Cabauw, Netherlands, and Hamburg, Munich, and Leipzig, Germany, after the strong eruptions of the Icelandic Eyjafjallajökul volcano in April and May 2010. A consistent picture in terms of photometer-derived fine- and coarse-mode AOTs and lidar-derived non-ash and ash extinction profiles is found. The good agreement between the fine- to coarse-mode AOT ratio and non-ash to ash AOT ratio (<10% difference) in several cases corroborates the usefulness of the new retrieval technique. The main phases of the evolution of the volcanic aerosol layers over central Europe from 16 April to 17 May 2010 are characterized in terms of optical properties and mass concentrations of fine fraction and ash particles. Maximum coarse-mode 500 nm AOTs were of the order of 1.0-1.2. Ash concentrations and column mass loads reached maximum values around 1500 μg/m3 and 1750 mg/m2, respectively, on 16-17 April 2010. In May 2010, the maximum ash loads were lower by at least 50%. A critical aspect of the entire retrieval scheme is the high uncertainty in the mass-to-extinction conversion for fresh volcanic plumes with an unknown concentration of particles with radii >15 μm.